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Science 6 June 2003:
Vol. 300. no. 5625, pp. 1553 - 1555
DOI: 10.1126/science.1083433
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Reports

Femtosecond Phase-Coherent Two-Dimensional Spectroscopy

Peifang Tian,1 Dorine Keusters,2 Yoshifumi Suzaki,3 Warren S. Warren2

Femtosecond phase-coherent two-dimensional (2D) spectroscopy has been experimentally demonstrated as the direct optical analog of 2D nuclear magnetic resonance. An acousto-optic pulse shaper created a collinear three-pulse sequence with well-controlled and variable interpulse delays and phases,which interacted with a model atomic system of rubidium vapor. The desired nonlinear polarization was selected by phase cycling (coadding experimental results obtained with different interpulse phases). This method may enhance our ability to probe the femtosecond structural dynamics of macromolecules.

1 Department of Electrical Engineering, Center of Ultrafast Laser Applications, Princeton University, Princeton, NJ 08544, USA.
2 Department of Chemistry, Center of Ultrafast Laser Applications, Princeton University, Princeton, NJ 08544, USA.
3 Department of Advanced Materials Science, Faculty of Engineering, Kagawa University, Takamatsu, Kagawa 761–0396, Japan.

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